x)Sr0.2Na0.4Sm0.4TiO3-em class="EmphasisTypeItalic">xLnAlO3 samples (where Ln stands for Nd, Pr and Sm, x?=?0.2-.3) were studied. The XRD result showed that the (1???em class="EmphasisTypeItalic">x)Sr0.2Na0.4Sm0.4TiO3-em class="EmphasisTypeItalic">xLnAlO3 (Ln?=?Nd, Pr and Sm) solid-solutions with single orthorhombic perovskite phase could be formed in the componential range of 0.2?≤?em class="EmphasisTypeItalic">x?≤?.3. With an increasing of Ln3+ content, the dielectric constant (ε r ) decreased due to the smaller dielectric?polarizability of LnAlO3 than that of Sr0.2Na0.4Sm0.4TiO3. With increasing x from 0.2 to 0.3, the quality factor (Q·f)?firstly?increased and?then?decreased for the specimens with PrAlO3, because the Q·f values were strongly depended on grain sizes. Moreover, either increasing the A-site bond valence or decreasing the B-site bond valence led to a decrease in the temperature coefficient of the resonant frequency (τ f). Typical values of ε r?~?52.7, Q·f?~?9700?GHz (at 4.33?GHz) and τ f?~?1.5?ppm/°C were obtained for the (1???em class="EmphasisTypeItalic">x)Sr0.2Na0.4Sm0.4TiO3-em class="EmphasisTypeItalic">xSmAlO3 (x?=?0.25) ceramic sintered at 1470?°C for 4?h." />